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Preparation of porous silica from natural chlorite via selective acid leaching and its application in methylene blue adsorption

选择性酸浸热活化天然绿泥石制备多孔二氧化硅材料

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Abstract

In this study, porous silica with high surface area was prepared through selective leaching of thermally activated chlorite in HCl solution. In the process, chlorite was activated by pre-calcining treatment, then activated components (MgO, Al2O3, and Fe2O3) were selectively leached by acid solution, resulting in the formation of nanopores in situ. The morphology, structure, surface area and pore-size distribution of the material were characterized by XRD, TG/DSC, 27Al MAS NMR, SEM, TEM and N2 adsorption-desorption isotherms. The highest specific surface area (SBET=333 m2/g) was obtained by selectively leaching the 600 °C calcined chlorite from 3 mol/L HCl at 90 °C for 2 h. The pore sizes and specific surface areas can be controlled by calcination and leaching conditions. The 27Al MAS NMR spectra of the samples revealed the relationship between structural transformation and the selective acid leaching properties of thermal-activated chlorite, demonstrating that AlVI transfers into AlV when chlorite changes into activated chlorite during thermal activation, and the coordinations of Al has a significant effect on acid solubility of chlorite. The as-prepared porous silica showed favorable adsorption abilities with capacity of 148.79 mg/g for methylene blue at pH of about 7 and temperature of 25 °C, indicating its promising potential in adsorption application.

摘要

在本研究中, 通过选择性酸浸热活化的绿泥石制备出高表面积的多孔二氧化硅材料. 首先, 绿泥石通过高温预煅烧处理转变为热活化绿泥石, 再利用盐酸溶液对其进行酸处理, 结构中的活性成分(MgO、Al2O3和Fe2O3)被选择性地浸出, 从而在活化绿泥石的片状氧化硅骨架上原位形成纳米孔道, 最终得到片状多孔二氧化硅材料. 热活化绿泥石制备多孔二氧化硅的最佳工艺条为:绿泥石煅烧温度为600 °C, 反应温度为90 °C, 盐酸浓度为3 mol/L, 反应时间为2 h, 得到最大比表面积为333 m2/g. 通过27Al MAS NMR研究了热处理过程中绿泥石中Al 的结构变化和选择性酸浸特性之间的关系, 发现绿泥石在热活化过程中Al 配位结构由AlVI转变为AlV, Al 的配位对绿泥石的酸溶性有重要影响. 通过静态吸附实验探讨了制备的多孔二氧化硅对亚甲基蓝有机染料的吸附性能, 在pH值为7、温度为25 °C时, 对亚甲基蓝的最大饱和吸附量为148.79 mg/g, 表明其对有机染料具有良好的吸附作用.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China

    Zhi-zeng Wang  (王志增), Qin-yi Zhao  (赵秦仪), Dong-yun Wang  (王冬云) & Chong Cui  (崔崇)

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  1. Zhi-zeng Wang  (王志增)
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Correspondence to Chong Cui  (崔崇).

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Project(51772153) supported by the National Natural Science Foundation of China

Contributors

WANG Zhi-zeng and CUI Chong provided the concept and edited the draft of manuscript. CUI Chong provided the field test conditions. WANG Zhi-zeng, ZHAO Qin-yi and WANG Dong-yun analyzed the results. WANG Zhi-zeng conducted the literature review and wrote the first draft of the manuscript. All authors replied to reviewers’ comments and revised the final version.

Conflict of interest

WANG Zhi-zeng, ZHAO Qin-yi, WANG Dong-yun and CUI Chong declare that they have no conflict of interest.

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Wang, Zz., Zhao, Qy., Wang, Dy. et al. Preparation of porous silica from natural chlorite via selective acid leaching and its application in methylene blue adsorption. J. Cent. South Univ. 29, 1173–1184 (2022). https://doi.org/10.1007/s11771-022-4970-4

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